Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 142, Issue 21, Pages 9752-9762Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c02633
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Funding
- Japan Society for the Promotion of Science (JSPS) [26102011, 15K21721, 17H06439, 19F19044, 18H03918]
- Deutsche Forschungsgemeinschaft [SPP 1928, HE 3543/31-1]
- Grants-in-Aid for Scientific Research [19F19044] Funding Source: KAKEN
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Visible-light-driven hydrogen (H-2) production from water is a promising strategy to convert and store solar energy as chemical energy. Covalent organic frameworks (COFs) are front runners among different classes of organic photocatalysts. The photocatalytic activity of COFs depends on numerous factors such as the electronic band gap, crystallinity, surface area, exciton migration, stability of transient species, charge separation and transport, etc. However, it is challenging to fine tune all of these factors simultaneously to enhance the photocatalytic activity. Hence, in this report, an effort has been made to understand the interplay of these factors and identify the key factors for efficient photocatalytic H-2 production through a structure-property activity relationship. Careful molecular engineering allowed us to optimize all of the above plausible factors impacting the overall catalytic activities of a series of isoreticular COFs. The present study determines three prime factors: light absorption, charge carrier generation, and its transport, which influence the photocatalytic H-2 production of COFs to a much greater extent than the other factors.
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